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Article Cite This: Environ. Sci. Technol. XXXX, XXX, XXX−XXX

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Effect of Stove Technology and Combustion Conditions on Gas and Particulate Emissions from Residential Biomass Combustion Deepika Bhattu,*,† Peter Zotter,‡ Jun Zhou,†,∥ Giulia Stefenelli,† Felix Klein,† Amelie Bertrand,†,§ Brice Temime-Roussel,§ Nicolas Marchand,§ Jay G. Slowik,† Urs Baltensperger,† Andre ́ Stephan Henry Prev́ ôt,† Thomas Nussbaumer,‡ Imad El Haddad,† and Josef Dommen*,† †

Laboratory of Atmospheric Chemistry, Paul Scherrer Institute, 5232 Villigen, Switzerland Bioenergy Research, Engineering and Architecture, Lucerne University of Applied Sciences and Arts, 6048 Horw, Switzerland § Aix Marseille Univ, CNRS, LCE, Marseille, France

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‡

S Supporting Information *

ABSTRACT: We have systematically examined the gas and particle phase emissions from seven wood combustion devices. Among total carbon mass emitted (excluding CO2), CO emissions were dominant, together with nonmethane volatile organic compounds (NMVOCs) (10−40%). Automated devices emitted 1−3 orders of magnitude lower CH4 (0.002−0.60 g kg−1 of wood) and NMVOCs (0.01−1 g kg−1 of wood) compared to batch-operated devices (CH4: 0.25− 2.80 g kg−1 of wood; NMVOCs: 2.5−19 g kg−1 of wood). 60−90% of the total NMVOCs were emitted in the starting phase of batch-operated devices, except for the first load cycles. Partial-load conditions or deviations from the normal recommended operating conditions, such as use of wet wood/wheat pellets, oxygen rich or deficit conditions, significantly enhanced the emissions. NMVOCs were largely dominated by small carboxylic acids and alcohols, and furans. Despite the large variability in NMVOCs emission strengths, the relative contribution of different classes showed large similarities among different devices and combustion phases. We show that specific improper operating conditions may even for advanced technology not result in the emission reduction of secondary organic aerosol (SOA) forming compounds and thus not reduce the impact of wood combustion on climate and health.

1. INTRODUCTION Increasing world energy demands (by 28% between 2015 and 2040)1 and identification of climatic effects from fossil fuel combustion accentuate the need for alternative energy sources. While wood is a potent renewable heat and energy source, it is also a significant source of primary particulate matter (PM) and secondary PM precursors, linked to adverse human health effects. The incomplete combustion products (ICPs) present in biomass smoke such as CO, CH4, nonmethane volatile organic compounds (NMVOCs), black carbon (BC), and organic aerosols (OA) deteriorate air quality.2−6 Studies showed the occurrence of DNA damage, lipid peroxidation and release of pro-inflammatory cytokines in lung cells can be caused by wood combustion emissions.7−11 After biogenic emissions,12 biomass burning is the second largest global contributor to atmospheric NMVOCs.13 Among the latter, a significant portion may be comprised of unidentified high molecular weight species,14−16 which are associated with the rapid formation of secondary organic aerosol (SOA),4,17−20 secondary NMVOCs and ground level ozone (O3).21−25 Extensive laboratory studies have focused on open biomass burning under fuel rich conditions for specific fuels,14,16,24,26−36 © XXXX American Chemical Society

but few studies are available on NMVOC emissions from residential wood combustion.37−49 Among them, most of the studies deployed offline sampling techniques such as Tedlar bags or PUF/Tenax-TA/DNPH-Silica/C18 Sep Pak cartridges or stainless steel canisters either for a complete combustion cycle or separately for different combustion phases and/or averaged over several batches. Such measurements are time-consuming and limited to a small range of compounds, for example, small carbonyls, sugars, polycyclic aromatic hydrocarbons, single ring aromatics38,40,41,47 in comparison to online instrumentation.43,45 In addition, a great majority has investigated photochemically aged emissions17,42,45,46,50−55 but very few examined the real-time influence of combustion conditions and technology on the emitted NMVOCs composition.56,57 Due to economic considerations and wood availability, residential wood heating is likely to persist in many parts of the world in the near future. Moreover, large incentives/ Received: Revised: Accepted: Published: A

September 6, 2018 January 14, 2019 January 16, 2019 January 16, 2019 DOI: 10.1021/acs.est.8b05020 Environ. Sci. Technol. XXXX, XXX, XXX−XXX

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Environmental Science & Technology subsidies to induce a shift from fossil to renewable energy production and the introduction of more stringent emission legislations58 have led to developments of combustion technology with varying configurations: from process control perspective, level of sophistication, and performance.59 The variations in the present investigation range from simple, low cost, manually operated technologies, that is, conventional single-stage combustion logwood stoves, to well-regulated, automated devices. In the past, the combustion quality and claimed reduced emissions are often compared focusing on commonly measured gas phase emissions (CO, total VOCs, and NOX) and total particle emissions and investigating only part of the combustion cycle. However, further information on the flue gas chemical composition is needed to evaluate the environmental impacts resulting from a shift toward more advanced technologies. The present study compares real-time emissions from different combustion technologies. First, we examine the interand intraburn variability of conventional emissions (CO, CH4, NO, eBC), POA and total NMVOCs among different tested devices to understand the effect of fuel and combustion parameters such as temperature, MCE and λ (see Section 3.1). Second, we evaluate the effect of stove technology on the evolution of emissions during the combustion cycle. We compare these emissions with those from automated devices tested in this study and literature values (see section 3.2). Third, we analyze the evolution of different classes of NMVOCs emission along the combustion cycle for different technologies in order to evaluate the performance of conventional and advanced technologies (Section 3.3). Fourth, we explored the dependence of individual NMVOC emission intensity, variability and chemical composition on combustion conditions including device and load type (first load/reloads), and combustion phases (Section 3.4).

conditions, and devices 3 and 4 were tested under partial-load. Logwood operated devices (2, 5, 6, and 7) were investigated for the complete combustion cycles with the first cycle referred to as “first load” and subsequent cycles, as “reloads”. The first load consisted of a cold start, flaming and burn-out phase, and reloads were comprised of a warm start, flaming and burn-out phase. More details on the specifications, operating conditions and combustion regimes of the tested devices are provided in the SI (Table S2 and Section S1). 2.2. Sampling Details. Details of the experimental setup and sampling strategy along with the operated instrumentation are given in SI Figure S1 and Section S2. Briefly, undiluted flue gas was measured through a thermally insulated heated line at 180 °C using a multigas analyzer system (Ultramat 23 Siemens; CO and NO: nondispersive infrared (NDIR) and O2: paramagnetic measurement) and a flame ionization detector (FID) with nonmethane cutter (109A, J.U.M Engineering: VOC and CH4). Only CH4 concentrations were used from FID. Further downstream, emissions were sampled after passing through two serially connected heated ejector dilutors (first at 180 °C and second at 100 °C), each with a dilution ratio of 1:10 (DI-1000, Dekati Ltd.). 2.3. Instrumentation. NMVOCs were measured by a proton transfer reaction time-of-flight mass spectrometer (PTRTOF-MS 8000, Ionicon Analytik G.m.b.H) operated with 6 and 10 s time resolution in 2015 and 2016, respectively. Sampled NMVOCs were protonated with H3O+ ions in the drift tube maintained at a drift voltage of 494 V, temperature of 90−100 °C, and pressure of 2.19−2.2 mbar resulting in E/N = 125−129 Td. For a quantitative determination60 of the VOC concentration (ppb), the mass resolution, mass accuracy and relative transmission function were determined by calibrating with common VOCs (m/z 33 to 181; Carbagas AG, Zurich, Switzerland) of known abundances (SI Figure S2 and Section S2.2). Data were analyzed with Tofware postprocessing software (version 2.5.3, TOFWERK AG, Thun, Switzerland). Reaction rate constants of the NMVOCs with H3O+ were used from the literature61 when available, otherwise a default rate constant of 2 × 10−9 cm3 molecule−1 s−1 was used. The high resolution of the PTR-TOF-MS allowed the molecular formula assignments. Tentative peak identification was based on literature reports on wood combustion emissions from both laboratory and field experiments (SI Table S3).31,37,42,43,62 Identified ions were classified according to their functional groups into 14 classes, including furans, hydrocarbons (HC), N-containing compounds (N is nitrogen atoms), polycyclic aromatic hydrocarbons (PAHs), single-ring aromatics (SRA), O-containing_acids (O is oxygen atoms), O-containing_alcohols, O-containing_C < 6 (where C is the number of carbon atoms), Ocontaining_C > 6, oxygenated aromatics_benzenediols/methoxy-phenols, oxygenated aromatics_methylphenols, oxygenated aromatics_oxygenated PAHs, and oxygenated aromatics_others, whereas the unidentified ions were congregated under “Others”. An aethalometer (AE 33, Magee Scientific) was used to determine the aerosol attenuation coefficients at seven wavelengths, from which the equivalent BC (eBC) mass concentration was retrieved.63 Primary organic aerosol (POA) mass concentration was obtained using an Aerodyne high resolution time-of-flight aerosol mass spectrometer (HR-TOF-AMS, Aerodyne Research Inc.). Details on additional measurements can be found elsewhere.36

2. MATERIALS AND METHODS 2.1. Tested Devices and Their Operating Conditions. Primary gas and particle phase emissions across six residential wood combustion devices (94 test burns) and one industrial boiler (six test runs) were characterized in real-time. We present the full suite of the current technology used in Swiss households with different fuel types and properties. The tested devices include the following (specified with manufacturing year and rated power): (a) two-stage combustion pellet operated devices: pellet boiler (device 1, 2004, 15 kW) and pellet stove (device 4, 2010, 2−6 kW), (b) two-stage combustion logwood operated devices: logwood boiler (device 2, 2007, 30 kW), advanced twostage combustion logwood stoves (device 6, 2013, 4.6 kW and device 7, 2016, 8 kW), (c) conventional single-stage combustion logwood stove (device 5, 2005, 6 kW), and (d) industrial wood chip moving grate boiler (device 3, 2013, 150 kW). Device 1, 3, and 5 were tested in 2015 and 2, 4, 6, and 7 in 2016. Fuels tested included wood pellets (EN certified, a quality standard developed by European Committee for Standardization) and wheat pellets, wood chips and logs made of beech wood with additional small pieces of soft wood (300−600 g) and fire kindling (20−30 g) as starters only during first loads. Supporting Information (SI) Table S1 presents the properties of fuels used in this study. Effect of different fuel properties was tested with fuel of different moisture contents (dry (∼13−16%) and wet (∼20−42%)) and fuel load conditions (normal and overload). Apart from their recommended combustion regimes, device 1 was also investigated during excess (λ++) and lack (λ--) of O2 B

DOI: 10.1021/acs.est.8b05020 Environ. Sci. Technol. XXXX, XXX, XXX−XXX

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Environmental Science & Technology

Figure 1. Combustion phase-specific gas phase (a: CO, b: CH4, c: POA and d: NMVOCs) EFs (g kg−1 of wood) vs MCE for seven combustion devices and their operating conditions (partial-/full load and excess (λ++), lack (λ−−), and optimum λ (λopt) condition) represented by different colored markers. Marker size refers to the combustion chamber temperature ranging from 150 to 1150 °C. The dashed black line in panel b−d is the fitted CO EF from panel a. The particle phase measurements in device 3 (moving grate boiler) refer to measurements before the electrostatic precipitator.

2.4. Data Analysis. Primary emission factors (EFs, mg kg−1 of wood given in SI Table S3) of conventional gases (CO2, CO, and CH4), NMVOCs (PTR-MS) and particle phase species EFx =

were calculated, following a carbon-mass-balance approach64 as described in eq 1.

Δx × fc Δ[CCO2] + Δ[CCO] + Δ[CCH4 ] + Δ[C VOC] + Δ[COC] + Δ[CeBC]

Here, Δx is the background-corrected concentration of the species of interest, and Δ[CCO2], Δ[CCO], Δ[CCH4], Δ[CVOC], Δ[COC], and Δ[CeBC] are the background-corrected carbon mass concentrations of carbon containing species in the flue gas. For the carbon fraction fc in the fuel a constant average value of the wood (0.46; SI Table S1) was assumed. Changes of fc over the burning cycle are expected to be small compared to the variability of the pollutant emissions and difficult to determine for all devices. OC is derived by dividing OM by the OM:OC ratio obtained from the AMS measurements. For automatic device 4 and devices with full combustion cycles (2, 5, 6, and 7), modified combustion efficiency (MCE = [CO2/(CO2 + CO)])65 is used to determine the combustion phases (start ≈ 0.974 and burn-out 95%) of the total emissions. Finally, we applied an unsupervised agglomerative twodimensional hierarchical clustering analysis (2D-HCA37,67−69) to the EFs of identified NMVOCs during different combustion phases to identify the main sources driving the chemical variation in the gas-phase. We have only considered devices 1, 2, 5, 6, and 7; devices 3 and 4 were excluded due to their extremely low EFs. More details on data preparation, clustering process,

C


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Figure 2. (a−d) Cumulative EFs of CO, CH4, NO, NMVOCs, and eBC in g kg−1 of wood emitted per consumed carbon mass fraction (calculated using eq 2) for logwood batch-operated devices (2 (n = 1), 5 (n = 9), 6 (n = 7), and 7 (n = 5)) and corresponding λ values (right axis) color coded with MCE. The orange, yellow, and gray shaded areas represent start, flaming and burn-out phase, respectively. For device 2 and 7, cumulative EFs represent first load and for device 5 and 6, average of both first load and reload combustion cycles. (e) Combustion phase-specific EFs of the above-mentioned species (stacked) from two-stage combustion pellet boiler and pellet stove, and wood chip operated industrial boiler (data available in SI Table S3) and cumulative EFs of the same species from the complete cycle of batch logwood operated devices (similar to the end points from panels a−d). As each set of experiment has one first load and several reloads (4−6), the effect of first loads in averaged cumulative EFs is not dominant in device 5 and 6. The particle phase measurements in device 3 (moving grate boiler) refer to measurements before the electrostatic precipitator. Averaged EFs for CO, NMVOCs, and CH4 for residential heating and laboratory field fires from literature are also compared. Specific EFs for CO, CH4, NMVOCs,41 or NMHCs (nonmethane hydrocarbons),45 POA or OC (organic carbon) and eBC from individual studies are provided in SI Figure S7.

automated (device 1, 3 and 4) devices were ∼10 times higher than for NMVOCs (Figure 1d). But due to the large variability in NMVOCs EFs (1 order of magnitude) of batch-operated devices, the comparison is not straightforward. Still, a similar decreasing trend with MCE was observed for NMVOCs. Overall, 50−90% of the total carbon mass (excluding CO2) was emitted as CO, whereas the rest consisted predominately of NMVOCs ( 6, oxygenated aromatics_benzenediols/methoxy-phenols and SRA increased with the evolution of combustion cycle and is in line with the observation of Sekimoto et al.,67 where “high- (500−800 °C)” temperature pyrolysis (e.g., depolymerization, fragmentation, and aromatization) led F


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NMVOCs classes to levels comparable to device 6. The combustion of wet wood (open symbols) in reloads and first load conditions increased all NMVOCs classes in device 6 but decreased them in device 5 (by ∼50%; except for PAHs). 3.4. NMVOC Species Variability with Combustion Conditions. NMVOCs fingerprints and their individual combustion phase-specific emission intensities were highly variable. As the data does not follow the normal distribution, rank transformation is applied before ANOVA (analysis of variance) analysis. Only a minor fraction of this variability could be explained by categorizing the data according to the differences in technology (22%) or together with the combustion phase information (12%). In contrast to the total NMVOCs EFs (shown in Figure 1), the EFs of individual compounds were only weakly dependent on MCE,79 λ or the combustion temperature. However, recently, Sekimoto et al.67 observed that combustion temperature is a better predictor of variability in open biomass burning NMVOCs emission profiles compared to MCE defined combustion phases. Our observations indicate that several parameters may concomitantly drive the overall variability observed in the NMVOCs chemical composition, and consequently, in this section we examine these parameters. Using 2D-HCA clustering analysis, the NMVOCs emissions could be classified into three major groups according to their composition (Figure 4b and c) and emission intensity (Figure 4a; also see SI Figure S9a for 2D-HCA analysis and SI Table S6 for more explanation). Decision tree classification algorithms further assisted in separation into groups and subgroups constituted on the basis of (1) combustion parameters, including device and load type (first load/reload), combustion phase, and conventional gas phase emissions (e.g., CO and CH4) and (2) main NMVOCs emitted. Group I exhibited high combustion phase-specific emissions of CH4 (∼1 g kg−1 of wood) and total NMVOCs (∼3 g kg−1 of wood) (Figure 4a and SI Figure S10b). Emissions were characterized by the relatively higher contribution of small oxygenated molecules, with acetic acid, propen-2-al, methyl vinyl ketone, acetaldehyde, methanol and formaldehyde as major species (Figure 4c). In contrast, Group II had low CH4 (0.10 g kg−1 of wood) and total NMVOCs (∼0.3 g kg−1 of wood) emissions. Group III featured similar levels of CH4 and NMVOCs as Group I but the NMVOCs emission profiles were significantly different. Emissions in Group III were characterized by the high abundance of HC (∼24%, compared to Group II [8.5%] and Group I [5%]) and higher molecular weight aliphatic oxygenated molecules (∼7% compared to Groups I and II [ 0.6 in each class, SI Figure S9c) into two distinct groups, Group I and III, while emission profiles classified in Group II were more variable (R ∼ 0.4, SI Figure S9c). Such grouping was not possible when the effects of single combustion parameters on the emissions were examined. Emissions from first loads and start phases of reloads were strictly classified in Group I (Figure 4d, SI Table S6) and characterized by high emissions of oxygenated NMVOCs (small aldehydes and acids, furans, and oxygenated aromatics). The significantly lower emissions from the burn-out phases were classified into Group II, with few exceptions of device 5 (conventional technology; Figure 4a and d). Flaming phase emissions from all devices were distributed among both groups (I and II), depending on the combustion conditions. High

to short and nonsubstituted aromatics and polycyclic aromatics (phenols, benzene, and PAHs) and “low-temperature ( 6 in all devices compared to device 5 scales roughly with the ratio of total NMVOCs (Figure 3e). The other classes were also reduced with different intensity and few exceptions. For example, in device 3, SRA, furans and hydrocarbons are by orders of magnitude more reduced than total NMVOCs and the O-containing class. On the other hand, emissions of SRA, PAHs and oxygenated PAHs in batchoperated device 7 are similar to those in device 5 while total NMVOCs is reduced by a factor of 2. This shows that devices with advanced technologies do not necessarily eliminate the problems arising from specific NMVOCs emissions. Despite a reduction of total NMVOCs, some critical compounds may not or only slightly be reduced keeping these devices still as a challenge for their use in the real world. Further, nonideal operation of device 1 (λ++) increased the emissions of all G


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distinguished from those of wood stoves (Ia and Ib) by the lack of a large number of hydrocarbon species, including alkenes/alkynes, PAHs (Cn > 11) and SRA (Cn > 8) as well as oxygenated aromatics (Cn > 7 or 8). When this device was operated under excess of O2 conditions (λ++), significant emissions of oxygenated NMVOCs were generated, resulting in the classification of these emissions into subgroup Ic (Figure 4). When this device was operated under optimal or fuel-rich combustion conditions (λopt and λ−−, respectively), emission profiles were distinctively classified into subgroup IIb due to lower emissions. The other lower emission profiles in Group II (IIa) from other devices (2, 5, and 6) are related to optimal flaming and burn-out conditions. The clustering revealed the unperceived differences between the emission fingerprints and could help relating these fingerprints to the combustion conditions classified into three groups with high and low CH4 and total NMVOCs emissions (SI Figure S9b). This suggests that CH4 can be used as an indicator for near-complete and in-complete combustion emissions, where at high CH4 levels the chemical composition of the emissions may significantly differ. Under those conditions, we need detailed chemical composition to predict the burden, the fate and the impacts of the emissions on the atmosphere.

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ASSOCIATED CONTENT

S Supporting Information *

The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/acs.est.8b05020. Details on wood combustion devices, sampling procedure and instrumentation, data analysis, fuel properties, specifications of combustion devices, cluster analysis, cumulative NMVOC EFs, fractional contribution of classified NMVOCs to the total NMVOC EFs, schematic of instrumental setup, transmission function of PTRTOF-MS, inconsistency coefficient in 2D-HCA, combustion phase-specific EFs of gas and particle phase species, evolution of EFs along the combustion cycle, comparison of averaged EFs among different technologies and operating conditions, comparison with literature studies, comparison of evolution of NMVCOs among different technologies, 2D-HCA dendrogram and EFs among different groups (PDF)

Figure 4. (a) Total EFs corresponding to a single combustion phase/ altered condition event from an individual device (x-axis), (b and c) fractional contribution of each NMVOCs class, and (d) cumulative number of samples/events over each device and combustion phase among different groups and further distinguished subgroups. The yellow, orange and green shaded areas represent Group I, Group II, and Group III, respectively.

Averaged EFs (conventional gas phase species and NMVOCs) (XLSX)

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emissions of oxygenated NMVOCs were observed during the flaming phases, when wet wood was used and when combustion temperature was lower. Emission profiles in Group III were characteristic of advanced wood stoves equipped with two-stage combustion technologies, especially emissions from device 7, revealing a clear dependence of the emission profiles on the technology used (Figure 4d). Further, Group I could also be further broken down into three different subgroups according to the technology. The start phases in the conventional (device 5) and the advanced wood stove (device 6) together with the logwood operated boiler (device 2) were classified into class Ia and Ib, respectively, because of their significantly higher benzenediols/methoxy-phenols emissions in the former (SI Figure S8). Emission profiles of the pellet boiler (device 1) were classified in the subgroup Ic and IIb, and were clearly

AUTHOR INFORMATION

Corresponding Authors

*(D.B.) E-mail: [email protected]. *(J.D.) E-mail: [email protected]. ORCID

Deepika Bhattu: 0000-0003-3597-190X Peter Zotter: 0000-0002-9274-9662 André Stephan Henry Prévôt: 0000-0002-9243-8194 Imad El Haddad: 0000-0002-2461-7238 Present Address ∥

(J.Z.) Graduate School of Global Environmental Studies, Kyoto University, Kyoto, 606−8501, Japan.

Notes

The authors declare no competing financial interest. H


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ACKNOWLEDGMENTS This study was financially supported by Swiss National Science Foundation (NRP 70 “Energy Turnaround”), the European Union’s Horizon 2020 research and innovation programme through the EUROCHAMP-2020 Infrastructure Activity under grant agreement no. 730997, and the Swiss Competence Centre for Energy Research SCCER BIOSWEET of the Swiss Innovation Agency Innosuisse.

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